Cetyltrimethyl ammonium bromid (CTMAB)-ZrP complexes that contained different amounts of CTMAB that intercalate into α-zirconium phosphate were successfully prepared while methylamine weakened the interlayer forces in α-zirconium phosphate. The CTMAB-ZrP samples were characterized by Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), and N2 sorption isotherm analysis. We discuss the arrangement of CTMAB in the interlayers of zirconium phosphate according to the characterization results. The results of the adsorption of phenol by CTMAB-ZrP showed that the amount of phenol adsorption depended on the content of CTMAB in the complex, the interlayer steric hindrance, and the pH value of the solution. The adsorption of phenol, 2-chlorophenol, 2,4-dichlorophenol, p-methylphenol, and 3,5dimethylphenol onto CTMAB-ZrP showed that the amount of adsorption correlated positively with the hydrophobicity of the phenols and it was not related to the acidity of the phenolic compounds. The sorption isotherms of phenol, 2-chlorophenol, and 2,4-dichlorophenol fit the Henry and Freundlich equations well. Therefore, the adsorption mechanism is mainly associated with the partition of different phenols in the organic phase of the intercalated CTMAB-ZrP.